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Metal sulfide demonstrated sluggish ionic transport kinetics due to the low electronic conductively, resulting larger volume expansion and even pulverize electrode during Li+ insertion/deinsertion. In this study, freestanding SnS nanoflower@carbon nanofiber (SnS@CNF) was prepared by the sol‐gel electrospinning of hydrothermal synthesized SnS2 nanoflower and carbonization. When direct used SnS@CNF as a binder‐free negative electrode for LIB, it delivered specific capacity of 564.4 mAh g−1@0.3 C after 450 cycles, and high rate capacities of 595, 465, 354, 267, 200, 129, 74, and 484 mAh g−1 at the current densities of 0.064, 0.1, 0.3, 0.6, 1.0, 1.5, 2.0, and 0.1 mA g−1, respectively. Such excellent electrochemical performance is attributed to the nanostructured conductive CNF network not only can buffer volume expansion and prevents the aggregation of active material, but also improve Li+ migration rates during the discharge (4.47×10−7 cm2 s−1) and charge (2.73×10−6 cm2 s−1) process. [ABSTRACT FROM AUTHOR]